Dissertations / Theses on the topic 'Quantum stark effect'

The effects of an applied bias in the longitudinal or growth direction on four In$\sb{\rm x}$Ga$\sb{\rm 1-x}$As-GaAs strained single quantum wells and three strained layer superlattices have been studied using photocurrent and electroreflectance spectroscopy at liquid helium temperature. Weak applied electric fields on the quantum well samples gives rise to a red quadratic shift to the lowest interband transition between the first confined electron (E1) and heavy-hole (H1) levels, the quantum confined Stark effect (QCSE). The magnitude of the QCSE increases with well width. This field dependence becomes subquadratic at high applied fields due to carrier accumulation on the low energy side of the wells. Superlattices with relatively small periods, i.e. 10 nm, exhibit interwell coupling giving rise to a miniband structure under flatband conditions. The application of an electric field removes the interwell coupling giving rise to a ladder like progression in energy for the interband transition energies, called Wannier Stark ladders. The measured exciton transition energies follow a linear field dependence given by the product of the Stark ladder index, the superlattice period, and the electric field. The low field behaviour is more complex due to the Coulomb interaction between the electrons and heavy-holes. The measured field dependent exciton transition energies for the quantum wells agree well with single particle model calculations, while for the superlattice samples the exciton Stark ladder calculations of Dignam and Sipe have yielded good agreement with the measured data.

Cette thèse porte sur la description théorique de processus dynamiques ultra-rapides de molécules polyatomiques et de leur contrôle par impulsions laser. Nous avons d’abord étudié la photochimie de l’aniline à l’aide de calculs de structure électronique. Nous avons d´écrit plusieurs régions clé des surfaces d’énergie potentielle et analysé ces résultats en relation avec les données expérimentales existantes. La photochimie de la pyrazine a été étudiée par des calculs de dynamiques quantique basés sur un Hamiltonien modèle incluant les quatre états électroniques excités de plus basse énergie et seize modes de vibration. Nous montrons que l’état sombre Au(nπ∗) joue un rôle important dans la dynamique de la molécule après photo-excitation. Un modèle simplifié à deux états et quatre modes a été utilisé pour étudier le contrôle par laser de la dynamique de la pyrazine photo-excitée. Nous proposons un mécanisme visant à augmenter la durée de vie de l’état B2u(ππ∗) en utilisant l’effet Stark induit par une impulsion laser intense non-résonante
The central subject of this thesis is the theoretical description of ultrafast dynamical processes in molecular systems of chemical interest and of their control by laser pulses. We first use electronic structure calculations to study the photochemistry of aniline. A umber of previously unknown features of the potential energy surfaces of the low-lying elec-tronic states are reported, and analyzed in relation with the experimental results available. We use quantum dynamics simulations, based on a model Hamiltonian including the four lowest excited electronic states and sixteen vibrational modes, to investigate the photochem-istry of pyrazine. We show that the dark Au(nπ∗) state plays an important role in the ultrafast dynamics of the molecule after photoexcitation. The laser control of the excited state dynamics of pyrazine is studied using a simplified two-state four-mode model Hamiltonian. We propose a control mechanism to enhance the lifetime of the bright B2u(ππ∗) state using the Stark effect induced by a strong non-resonant laser pulse. We finally focus on the laser control of the tunneling dynamics of the NHD2 molecule, using accurate full-dimensional potential energy and dipole moment surfaces. We use simple effective Hamiltonians to explore the effect of the laser parameters on the dynamics and design suitable laser fields to achieve the control. These laser fields are then used in MCTDH quantum dynamics simulations. Both enhancement and suppression of tunneling are achieved in our model

The quantum confined Stark effect (QCSE) and ultrafast absorption dynamics near the bandedge have been investigated in p-i-n waveguides comprising quantum confined heterostructures grown on GaAs substrates, for emission at 1.3um. The materials are; isolated InAs/InGaAs dot-in-a-well (DWELL) quantum dots (QD), bilayer InAs quantum dots and GaInNAs multiple quantum wells (MQW). The focus was to investigate these dynamics in a planar waveguide geometry, for the purpose of large scale integration in optical systems. Initial measurements of the QCSE using photocurrent measurements showed a small shift for isolated QDs whilst a significant shift of 40nm (at 1340nm) was demonstrated for bilayer dots, comparable to that of GaInNAs MWQ (30nm at 1300nm). These are comparable to InP based quaternary multiple quantum wells used in modulator devices. With the use of a broadband continuum source the isolated quantum dots exhibit both a small QCSE (15nm at 1280nm) and minimal broadening which is desirable for saturable absorbers used in monolithic modelocked semiconductor lasers (MMSL). A robust experimental set-up was developed for characterising waveguide modulators whilst the electroabsorption and electro-refraction was calculated (dn=1.5x10⠻³) using the Kramers-Kronig dispersion relation. Pump probe measurements were performed at room temperature using 250fs pulses from an optical parametric oscillator (OPO) on the three waveguide samples. For the isolated QDs ultrafast absorption recovery was recorded from 62ps (0V) to 700fs (-10V and the shortest times shown to be due to tunneling. Additionally we have shown good agreement of the temperature dependence of these dots and the pulse width durations from a modelocked semiconductor laser using the same material. Bilayer QDs are shown to exhibit ultrafast absorption recovery from 119ps (0V) to 5ps (-10V) offering potential for applications as modelocking elements. The GaInNAs multiple quantum wells show absorption recovery of 55ps (0V), however under applied reverse bias they exhibit long lived field screening transients. These results are explained qualitatively by the spatial separation of electrons and holes at heterobarrier interfaces.

In this work optical properties of two dimensional quantum well structures are studied. Variational calculation of the eigenstates in an isolated quantum well structure with and without the external electrical field is presented. At weak fields a quadratic Stark shift is found whose magnitude depends strongly on the finite well depth. It is observed that under external electrical field, the asymmetries due to lack of inversion symmetry leads to higher order nonlinear optical effects such as second order optical polarization and second order optical susceptibility.

Semiconductor nanowires have attracted considerable attention as possible source for lasers and optical storage media. We report the fabrication and optical characterization of ZnO and CdS nanowires. The former are produced by electrochemical deposition of Zn inside nanoporous alumina films containing regimented arrays of 10nm, 25nm and 50 nm diameter pores, followed by room temperature chemical oxidization. Fluorescence spectroscopy shows different characteristics associated with different sample diameter. The 50 nm ZnO nanowires show an exciton recombination peak and an additional peak related to the deep trap levels. 25 nm ZnO nanowires show a only the exciton recombination peak, which is red shifted, possibly due to quantum confined Stark effect associated with built in charges in the alumina. This feature can be exploited to produce light emitting devices whose frequency can be modulated with an external electric field. Such devices could be novel ultra-violet frequency modulators for optical communication and solar blind materials. In addition, we have investigated fluorescence spectra of 10-, 25- and 50-nm diameter CdS nanowires (relative dielectric constant = 5.4) self assembled in a porous alumina matrix (relative dielectric constant = 8-10). The spectra reveal peaks associated with free electron-hole recombination. The 10-nm wire spectra show an additional lower energy peak due to exciton recombination. In spite of dielectric de-confinement caused by the insulator having a higher dielectric constant than the semiconductor, the exciton binding energy increases almost 8-fold from its bulk value in the 10 nm wires. This increase is most likely due to quantum confinement accruing from the fact that the exciton Bohr radius (~5 nm) is comparable to or larger than the wire radius, especially if side depletion is taken into account. Such an increase in the binding energy could be exploited to make efficient room temperature luminescent devices in the visible range.

Les paires d'ions sont omniprésentes dans la nature, depuis l'eau de mer, les aérosols, jusqu'aux organismes vivants. Elles influencent les propriétés des solutions concentrées en ions, et jouent ainsi un rôle majeur dans divers réactions chimiques et processus biologiques. Cependant, la caractérisation des paires d’ions se heurte à une double difficulté : d'une part, plusieurs types de paires coexistent, et d'autre part, ce sont des espèces transitoires en solution. Dans ce contexte, ce travail présente plusieurs études menées selon trois axes de recherche principaux grâce à une approche originale en phase gazeuse, puis en solution. Le premier axe consiste à étudier les effets du champ électrique produit par la paire d’ions sur la spectroscopie d’un chromophore UV en phase gazeuse (effets Stark). Les groupes ioniques sont capables de produire un champ électrique suffisamment élevé pour induire des effets Stark électroniques significatifs sur un chromophore UV situé à proximité. Cette étude est menée sur des systèmes modèles de formule générale (C₆H₅-(CH₂)n₋COO⁻,M⁺) avec M = Li, Na, K, Rb, Cs et n = 1-3, permettant de faire varier le champ électrique ressenti par le chromophore UV. Ces différents systèmes sont étudiés en phase gazeuse par spectroscopie UV combinée à des calculs de chimie quantique, ainsi que par des expériences de spectroscopie IR sélective en conformation. Grâce à cette approche, des attributions conformationnelles précises peuvent être proposées pour des transitions électroniques séparées de quelques cm-1, sur la base de l’analyse des effets Stark observés sur le spectre UV, sans recourir à la spectroscopie IR, ni aux calculs de fréquences. Il s’agit ensuite de comprendre les effets d’environnement sur les paires d’ions par des expériences de microsolvatation en phase gazeuse. La paire d’ions d’acétate de sodium [CH₃-COO⁻,Na⁺] est étudiée pour la première fois dans un complexe trimère avec le p-xylène par spectroscopie IR. Des expériences de microhydratation sont ensuite réalisées sur des paires d’ions chargées ([CH₃-COO⁻,M²⁺] ; M = Ca, Ba), mettant en évidence deux comportements différents en fonction de la nature du dication. Les différentes expériences montrent que la signature IR du groupement carboxylate est sensible à son environnement proche, mais également à l’environnement du cation qui lui est apparié. Le dernier axe consiste à détecter et identifier les structures formées par les ions dans les solutions électrolytiques par spectroscopies IR et RX. Une première analyse est effectuée sur des solutions électrolytiques ([CH₃-COO⁻,M⁺] ; M = Li, Na et K) par spectroscopie IR-TF en variant la concentration en ions. Une étude théorique est ensuite réalisée dans l’objectif de proposer un spectre théorique pour chaque type de paires, et de les confronter aux spectres expérimentaux en solution. L’approche repose sur le calcul de la signature IR de paires ([CH₃-COO⁻,M⁺] ; M = Li, Na, K, Rb et Cs) et de l’anion libre, entourés successivement de molécules d’eau explicites décrites au niveau chimie quantique, puis au niveau champ de force et enfin par un modèle de solvant continu. Pour chaque type de paires, des familles spectroscopiques compatibles avec les données expérimentales sont identifiées. Cette approche originale ouvre la voie vers l’identification des structures supramoléculaires dans les solutions électrolytiques. Enfin, la première expérience FZRET en micro-jet liquide est réalisée sur une solution d’acétate de potassium, donnant accès à une mesure de la distribution des distances entre cations et anions appariés. Au cours de ces études, différentes méthodes sont employées allant de l’expérience à la théorie, de la phase gazeuse à la solution. Cette thèse illustre la nécessité de combiner plusieurs méthodes afin d’obtenir des données complémentaires permettant une meilleure caractérisation de l’organisation supramoléculaire des ions et de leur environnement
Ion pairs are ubiquitous in nature, from sea water, aerosols, to living organisms. They influence the properties of concentrated ion solutions, and thus play a crucial role in various chemical reactions and biological processes. However, the characterization of ion pairs faces some difficulties: on one hand, several types of pairs coexist, and on the other hand, they are transient species in solution. In this context, this work presents several studies carried out according to three main research studies, backed by an original approach in the gas phase, and then in solution. Firstly, the effects of the electric field produced by the ion pair on the UV spectroscopy of a chromophore in gas phase (Stark effects) are studied. The ion groups can produce an electric field high enough to induce significant electronic Stark effects on a nearby UV chromophore. This study is conducted on model systems (C₆H₅-(CH₂)n-COO⁻,M⁺) with M = Li, Na, K, Rb, Cs and n = 1-3, allowing to vary the electric field experienced by the UV chromophore. These different systems are studied in the gas phase by UV spectroscopy combined with quantum chemistry calculations, as well as by conformation selective IR spectroscopy. Based on the analysis of the electronic Stark effects, precise conformational assignments can be proposed for electronic transitions separated by a few cm-1, without resorting to IR spectroscopy, or frequency calculations. The next study is focused mainly on understanding the environmental effects on ion pairs by microsolvation experiments in gas phase. The pair of sodium acetate ions [CH₃-COO⁻,Na⁺] is studied for the first time in a trimer complex with p-xylene by IR spectroscopy. Microhydration experiments are then carried out on charged ion pairs ([CH₃-COO⁻,M²⁺]; M = Ca, Ba), highlighting two different behaviours depending on the nature of the cation. The final research is to detect and identify the structures formed by the ions in electrolytic solutions by IR and RX spectroscopy. The first experiment is carried out on electrolytic solutions ([CH₃-COO⁻,M⁺]; M = Li, Na and K) by TF-IR spectroscopy by varying the ion concentration. A theoretical study is then carried out in order to propose a theoretical spectrum for each type of pair, and to confront them with experimental spectra in solution. The approach is based on the calculation of the IR signature of pairs ([CH₃-COO⁻,M⁺]; M = Li, Na, K, Rb and Cs) and free anion in solution, where the first solvation layer were described at the quantum level, followed by a solvent continuum. For each type of pair, spectroscopic families, consistent with the experimental data, are identified. This original approach paves way to the identification of supramolecular structures in electrolytic solutions. Finally, the first FZRET experiment in liquid micro-jet is carried out on a potassium acetate solution, providing access to a measurement of the distance distribution between cations and paired anions.In these studies, different methods are used ranging from experiment to theory, from the gas phase to solution. This work illustrates the need to combine several methods in order to obtain additional data and allow a better characterization of the supramolecular organisation of ions and their environment

La photo-isomérisation par ouverture de cycle du benzopyrane a été étudiée à l'aide de la méthode MCTDH (Multi-Configuration Time-Dependent Hartree). Nous avons introduit différentes stratégies pour contrôler la conversion du benzopyrane en mérocyanine à l'aide d'impulsions laser. Nous avons utilisé un modèle pour le potentiel électronique à six dimensions développé dans le cadre d'un travail antérieur. Le modèle repose sur une généralisation des Hamiltoniens modèles standards pour les couplages vibroniques et utilise les six coordonnées les plus importantes pour le processus. Le principal objectif est de fournir des stratégies de contrôle qui pourront être utilisées par les expérimentateurs par la suite. Plus précisément, nous avons proposé: (i) une technique de type pompe-sonde pour contrôler la photostabilité, (ii) une stratégie en deux étape avec une préexcitation vibrationnel du système,(iii) une stratégie reposant sur un contrôle par effet Stark induit par un laser non-résonant
The ring-opening photoisomerization of benzopyran, which occurs via a photochemical route involving a conical intersection,has been studied with quantum dynamics calculations using the multi-configuration time-dependent Hartree method (MCTDH). We introduce a mechanistic strategy to control the conversion of benzopyran to merocyanine with laser pulses. We use asix-dimensional model developed in a previous work for the potential energy surfaces (PES) based on an extension of thevibronic-coupling Hamiltonian model (diabatization method by ansatz), which depends on the most active degrees of freedom. The main objective of these quantum dynamics simulations is to provide a set of strategies that could help experimentalists tocontrol the photoreactivity vs. photostability ratio (selectivity). In this work we present:(i) a pump-dump technique used tocontrol the photostability, (ii) a two-step strategy to enhance the reactivity of the system: first, a pure vibrational excitation inthe electronic ground state that prepares the system and, second, an ultraviolet excitation that brings the system to the firstadiabatic electronic state; (iii) finally the effect of a non-resonant pulse (Stark effect) on the dynamics

Nous presentons le developpement et l'etude d'un dispositif photorefractif a puits quantiques ainsi que les mecanismes physiques fondamentaux associes a ce type de composants. La structure de bande de type i pour les trous lourds et de type ii pour les trous legers permet une mesure precise du decalage de bande de valence de cdte/cd#. #7#2zn#0#. #3#8te egal a +11% 2%. Cette situation particuliere produit une degenerescence entre niveaux de trous lourds et trous legers. Dans les puits peu profonds, l'exciton leger est de type i grace au potentiel coulombien exerce par l'electron sur le trou leger. Sous champ electrique, nous mettons en evidence une transition type i-type ii de l'exciton leger. Lorsque l'energie de liaison de l'exciton augmente, la constante dielectrique et l'interaction des excitons avec le reseau diminuent. L'observation de complexes exciton-phonon a basse temperature et leur disparition progressive lorsque l'energie de liaison augmente est favorable a cette interpretation. Une absorption excitonique intense a temperature ambiante est cependant observee lorsque l'energie de liaison est proche ou superieure a l'energie des phonons optiques longitudinaux. En nous fondant sur ces resultats, nous avons developpe un dispositif photorefractif a partir d'une diode schottky et nous avons mesure un rendement de diffraction proche de la valeur theorique. Un maintien du reseau de diffraction inscrit de quelques microsecondes necessite un blocage des porteurs qui ecrantent localement le champ applique. L'introduction de barrieres de potentiel en cdmgznte bloquent efficacement le mouvement perpendiculaire des electrons. Un modele qualitatif et des simulations numeriques permettent de cerner le comportement dynamique du dispositif. La diffusion laterale a l'interface est acceleree par le gradient de potentiel entre zones eclairees et sombres et limite le temps de maintien du reseau. Par des mesures de type pompe-sonde, nous avons determine la diffusion laterale et sa dependance avec le champ applique

Ce travail de thèse porte sur l'étude des propriétés optiques et électroniques des puits quantiques de GaN / AlGaN grâce à des techniques classiques de réflectivité résolue en angle et de photoluminescence, ainsi qu'avec la technique de photoluminescence résolue temporellement. Les expériences de photoluminescence en régime continu ont permis d'estimer les énergies des transitions excitoniques qui sont également accessibles en réflectivité. Ces techniques ont ainsi permis de mettre en évidence l'effet Stark dans les puits quantiques GaN / AlGaN. L'effet Stark sur les énergies de transition est cohérent avec la théorie des fonctions enveloppes. Les spectres de réflectivité permettent d'accéder à la force d'oscillateur des excitons grâce à leur modélisation par le formalisme des matrices de transfert, prenant en compte les phénomènes d'élargissement homogène et inhomogènes des transitions optiques. Enfin, les mesures de photoluminescence résolue en temps en fonction de la température, ont également permis d'extraire la force d'oscillateur qui est inversement proportionnelle au temps de recombinaison radiative. Cette étude a également permis de mettre en évidence l'effet Stark responsable de la diminution de la force d'oscillateur en fonction de l'épaisseur du puits quantique mais aussi en fonction de la composition d'aluminium. L'augmentation de l'épaisseur du puits entraîne une diminution du recouvrement des fonctions d'onde, et une augmentation de la composition d'aluminium intensifie le champ électrique et diminue également le recouvrement des fonctions d'onde.

InGaN based light emitting devices operating in the blue and near UV spectral regions are commercialized and used in many applications. InGaN heterostructures experience compositional inhomogeneity and thus potential fluctuations, such that regions of higher indium composition are formed and correspond to lower potentials. The indium rich regions form localization centers that save carriers from non-radiative recombination at dislocations, thus despite the large defect density, their quantum efficiency are surprisingly large. However, the conventional c-plane InGaN QWs suffer from high internal piezoelectric and spontaneous fields. These fields are detrimental for the performance of such structures as they lead to the quantum confined stark effect causing red-shift of the emission as well as reducing the electrons and holes wavefunctions overlap, thereby reducing the radiative recombination rate. However, growth of InGaN QWs on semipolar and nonpolar planes greatly reduced the polarization fields. Semipolar and nonpolar QWs experience an outstanding property which is polarized luminescence, opening a new frontier for applications for InGaN emitting devices. While nonpolar QWs have larger degree of polarized emission than semipolar QWs, semipolar QWs can emit in longer wavelengths due to their higher indium uptake. In this thesis, semipolar 20¯21 and nonpolar m-plane InGaN/GaN QWs were investigated. Photoluminescence, spectral and polarization dynamics were all studied in order to form a whole picture of the carrier dynamics in the QWs. Time resolved photoluminescence measurements were conducted for following carriers distribution between extended and localized states. Both the semipolar and nonpolar samples showed efficient luminescence through short radiative recombination times, as well as carrier localization in lower potential sites after thermal activation of excitons. Carrier localization was found to be benign as it didn’t degrade the performance of the samples or decrease the polarization ratio of their emission. However, the structures showed modest potential variations with the absence of deep localization centers or quantum dots. High polarization ratios were measured for both samples, which is well-known for nonpolar QWs. The high polarization ratio for the semipolar sample is of great importance, thus semipolar 20¯21 QWs should be considered for longer wavelength emitters with highly polarized spontaneous emission.

This PhD thesis is devoted to study electro-optic properties of Gemanium/Silicon-Germanium (Ge/SiGe) multiple quantum wells (MQWs) for light modulation, detection, and emission on Si platform. It reports the first development of high speed, low energy Ge/SiGe electro-absorption modulator in a waveguide configuration based on the quantum-confined Stark effect (QCSE), demonstrates the first Ge/SiGe photodiode with high speed performance compatible with 40 Gb/s data transmission, and realizes the first Ge/SiGe light emitting diode based on Ge direct gap transition at room temperature. Extensive DC and RF measurements were performed on each tested prototype, which was realized using the same epitaxial growth and fabrication process. Simple theoretical models were employed to describe experimental properties of the Ge/SiGe MQWs. The studies show that Ge/SiGe MQWs could potentially be employed as a new photonics platform for the development of a high speed optical link fully compatible with silicon technology.

Die vorliegende Arbeit beschäftigt sich mit optischen Untersuchungen von MBE-gewachsenen hexagonalen Gruppe-III-Nitridheterostrukturen. Dafür wird die Photolumineszenz von InGaN/GaN- und GaN/AlGaN-Mehrfachquantengrabenstrukturen umfangreich zeitintegriert und zeitaufgelöst studiert. Die Proben unterscheiden sich in den Dicken der Quantengräben und Barrieren (InGaN) bzw. in der kristallografischen Orientierung (AlGaN). Als Ergebnis der großen, für das Materialsystem charakteristischen, elektrostatischen Felder zeigen die konventionell [0001]-orientierten Heterostrukturen eine verringerte Übergangsenergie und längere Lebensdauern mit zunehmender Quantengrabenbreite und höherem Indiumgehalt in den Gräben. Der beobachtete Einfluss des Quantumconfined Stark-Effektes (QCSE) auf diese Größen kann auch durch Modellrechnungen quantitativ gezeigt werden. In der Arbeit wird erstmals eine umfangreiche optische Charakterisierung einer neuartigen [1-100]-orientierten GaN-Heterostruktur auf Gamma-LiAlO2 geboten. Zum Vergleich wird das Verhalten einer identisch aufgebauten, [0001]-orientierten Struktur auf SiC ebenfalls diskutiert. Die (1-100)-Probe ist in Wachstumsrichtung frei von elektrostatischen Feldern und unterscheidet sich damit deutlich von den herkömmlichen Nitridstrukturen mit [0001]-Orientierung, deren interne Felder im MV/cm-Bereich liegen. Die spektrale Lage der Photolumineszenz bei geringen Anregungsdichten bestätigt die Flachbandsituation in der Probe. Aufgrund des bei dieser Probe nicht auftretenden QCSE ist hier eine deutlich verkürzte Lebensdauer festzustellen. Entsprechend der Auswahlregeln für hexagonales GaN weist die [1-100]-orientierte Probe eine sehr starke Polarisation der Photolumineszenz bezogen auf die Lage der [0001]-Achse auf. Die geringe Abweichung des ermittelten Polarisationsgrades von der, für A-Exzitonen in Volumen-GaN zu erwartenden, totalen Polarisation kann durch das Konfinement in den Quantengräben erklärt werden. Ein Schwerpunkt der Arbeit ist die Untersuchung der Rekombinationsmechanismen der Proben in Abhängigkeit von der induzierten Ladungsträgerdichte. Diese wird in einem Bereich von sehr geringer Dichte bis über die Mottdichte variiert. Eine Abschirmung der elektrostatischen Felder mit zunehmender Ladungsträgerdichte wird festgestellt. Dabei kann bei einer InGaN/GaN-Probe mit 3.1 nm breiten Gräben gezeigt werden, dass neben den internen piezoelektrischen Feldern die in der Literatur diskutierte Lokalisation von Exzitonen an Stöchiometrieschwankungen des Quantengrabens entscheidend die Rekombinationsdynamik in der Probe beeinflusst. Dies spiegelt sich in einer Abhängigkeit der Quantengrabeneigenschaften von den Anfangsbedingungen des Abklingprozesses und damit einem nicht existierenden allgemein gültigen Zusammenhang zwischen der Lebensdauer und der Ladungsträgerdichte wider. Die zeitaufgelösten Lumineszenzspektren der InGaN/GaN-Strukturen zeigen als Folge der mit höheren Ladungsträgerdichten zunehmenden Abschirmung eine verringerte Lebensdauer durch die vergrößerte Überlappung von Elektron- und Lochwellenfunktionen. Aufgrund der wieder abnehmenden Abschirmung während des Rekombinationsprozesses verändert sich die Lebensdauer im Laufe der Zeit. Gleichzeitig kommt es zu einer Verringerung der Übergangsenergie des Lumineszenzmaximums durch den weniger abgeschirmten QCSE. Die zeitintegrierten Photolumineszenzspektren zeigen ebenfalls eine deutliche Abhängigkeit von der Anregungsdichte. Während bei der feldfreien (1-100)-Probe keine Kompensationseffekte erwartet werden, weisen die Resultate für die konventionellen Proben auf einen, die Ladungsträgerdichte wesentlich beeinflussenden Effekt hin. Die Abhängigkeit der Intensität der Photolumineszenz von der Ladungsträgerdichte deutet ab einer bestimmten Anregungsdichte auf einen zusätzlichen Prozess, welcher die Ladungsträgerdichte reduziert, sich aber nicht im Lumineszenzspektrum widerspiegelt. Als Erklärung dafür wird die Absorption von stimulierter Emission im Substrat oder in der Pufferschicht angenommen. Bei den InGaN-Proben schiebt die Übergangsenergie mit höheren Dichten zu größeren Energien und nähert sich bis 10e5 W/cm2 einem Sättigungswert an. Dieser Wert entspricht trotz Dichten oberhalb der Mottdichte noch nicht der Flachbandsituation bei vollständig kompensierten internen Feldern. Als Ursache dafür wird der genannte, bei hohen Ladungsträgerdichten einsetzende Konkurrenzprozess gesehen. Bei den GaN/AlGaN-Proben kann im untersuchten Bereich der Anregungsdichte keine spektrale Verschiebung im Photolumineszenzspektrum festgestellt werden. Zum ersten Mal werden experimentelle Untersuchungen zur stimulierten Emission einer [1-100]-orientierten GaN-Probe durchgeführt und das optische Gewinnspektrum analysiert. Die Messungen zeigen einen maximalen Nettogewinn von ca. 50 1/cm. Aus der rechnerischen Analyse der Modenausbreitung lässt sich dafür ein Materialgewinn für GaN(1-100) von 1.1x10e4 1/cm ableiten. Die Ergebnisse zeigen außerdem, dass die Rekombination eines Elektron-Loch-Plasmas der Mechanismus für die stimulierte Emission ist. Dies entspricht dem überwiegenden Teil der in der Literatur veröffentlichten Beobachtungen für [0001]-orientierte Nitridstrukturen. Ein direkter Vergleich mit der parallel untersuchten GaN/AlGaN(0001)-Probe ist aufgrund der starken Substratabsorption nicht möglich. Es zeigt sich, dass für [1-100]-orientierte GaN-Heterostrukturen gute Ausgangsbedingungen für die Realisierung von Laserdioden gegeben sind. Zu den untersuchten Heterostrukturen wird die Wellenführung in den Proben simuliert. Bei den auf SiC gewachsenen Schichten werden die sich ausbreitenden Moden wegen des deutlich höheren Brechungsindexes des Substrates vornehmlich dort geführt. Die Überlappung der Moden mit dem aktiven Schichtpaket ist äußerst gering. Es ist für die Proben auf SiC kein optischer Gewinn zu erwarten. Die [1-100]-orientierte GaN/AlGaN-Probe besitzt eine deutlich bessere Wellenführung, da das LiAlO2 einen vergleichsweise kleinen Brechungsindex besitzt. Es wird ein Zusammenhang zwischen experimentell ermitteltem optischen Gewinn und dem Materialgewinn gebildet und das Ergebnis mit Rechnungen aus der Literatur verglichen. Ein Vorschlag für eine optimierte Wellenführung in allen untersuchten Proben wird gegeben.
In this thesis, the optical properties of molecular beam epitaxy grown hexagonal group-III nitride heterostructures are studied. The photoluminescence (PL) characteristics of InGaN/GaN and GaN/AlGAN multiple quantum well structures are investigated by time-integrated and time-resolved measurements. The analyzed specimens differ in the width of the quantum wells and barriers (InGaN) and in the crystallographic orientation (AlGaN), respectively. As a result of the large characteristic electrostatic fields, conventional [0001]-oriented heterostructures show a reduced transistion energy and longer lifetimes with increasing well width and higher Indium content in the wells. The observed impact of the Quantum Confined Stark Effect (QCSE) on these quantities is quantitatively shown in model calculations. In this work, a first extensive optical characterization of a novel [1-100]-oriented GaN heterostructure grown on Gamma-LiAlO2 is presented. For comparison, an identically designed [0001]-oriented structure on SiC is discussed. The (1-100)-grown specimen is free of electrostatic fields along the growth direction and shows a significant different behavior than conventional [0001]-oriented nitrides with internal fields of several MV/cm. The existing flat band conditions are confirmed by the spectral position of the PL at low excitation densities. Due to the non-existing QCSE at this specimen an significantly reduced lifetime is observed. A strong polarization of the PL is observed for the [1-100]-oriented sample, following the selection rules for hexagonal GaN. The small deviation of the degree of polarization from unity, which is expected in bulk GaN, is attributed to the quantum confinement in the heterostructures. One main topic of this thesis is the analysis of the recombination mechanisms of the specimens depending on the induced carrier density. The carrier density is varied from very low upto densities above the mott density. A screening of the electrostatic fields is observed with increasing carrier density. It is shown, that an InGaN/GaN heterostructure with a well width of 3.1 nm not only is influenced by internal piezoelectric fields but also the localization of excitons at stoichiometric inhomogenities in the quantum well is playing an important role for the recombination dynamics of the structure. This can be seen in the dependence of the decay process on the starting conditions. No general correlation is existing between lifetime and carrier density. Time-resolved PL measurements on InGaN/GaN heterostructures show a reduced lifetime due to an increased overlap of the electron and hole wave functions as a result of the increased screening at increasing carrier densities. During the recombination process the screening decreases again and the lifetime is changed with time. Simultaneously the transistion energy of the PL maximum is reduced by the less screened QCSE. A distinct dependence of the time-integrated PL spectra on the excitation density was also found. While there are no compensation effects expected at the (1-100) structure, which is free of electrostatic fields, the results for the conventional specimens point to an effect which influences the carrier density essentially. The dependence of the PL intensity on the carrier density points to an additional process, which comes into play at a special excitation density. This process reduces the carrier density but is invisible in the PL spectra. As an explanation we assume, that light of stimulated emission is absorbed either in the substrate or in the buffer layer. The transistion energy of the InGaN structures increases with increasing excitation density and reaches a saturation energy at a density of 10e5 W/cm2. Although this density is larger than the mott density, the transistion energy is not equivalent with a transition energy at flat band conditions. The origin of the observed effect is assumed to be the rival process, mentioned above, which comes into play at high carrier densities. For the GaN/AlGaN heterostructures no spectral shift of the PL was observed within the variation of excitation density. For the very first time, the stimulated emission of an [1-100]-oriented GaN structure was analyzed. A maximum netto gain of 50 1/cm was observed. From calculations of the mode propagation, a material gain of 1.1x10e4 1/cm is derived for GaN(1-100). Additionally from the results follows that the recombination of an electron-hole-plasma is the mechanism of the stimulated emission. This is in accordance with most of the published observations for [0001]-oriented GaN heterostructures. A direct comparison of both, the [1-100]-oriented specimen and the GaN/AlGaN(0001) structure, which was investigated parallel, was not possible. The reason for that is the strong absorption of the SiC substrate of the latter mentioned structure. It is generally shown, that [1-100]-oriented GaN heterostructures offers good starting conditions to realize laser diodes. The wave guiding was simulated for all of the used specimens. At structures grown on SiC the propagating modes are mainly guided in the substrate due to the larger refractive index of SiC with respect to GaN. The overlap of the amplified mode and the active layer is very small. No optical gain is expected for these structures. The [1-100]-oriented GaN/AlGaN structure shows a significantly improved wave guiding, due to the small refractive index of LiAlO2 in comparison with GaN. A correlation between the experimentally observed optical gain and the material gain is formed and the results are compared with the literature. A suggestion for an optimized wave guiding in all investigated specimens is given.

La compréhension approfondie des interactions au sein des matériaux luminescents sous excitation revêt une importance cruciale pour le développement de dispositifs optoélectroniques. Les matériaux de faibles dimensions présentent des propriétés optoélectroniques uniques, résultant des effets quantiques et du confinement spatial.L'approche pour l'analyse des propriétés optoélectroniques des nanomatériaux s'est caractérisée par une démarche polyvalente, explorant différentes méthodes intégrées au microscope à transmission électronique à balayage (STEM). Grâce à une source d'électrons accélérée à 60 keV, cette étude a échappé aux limitations de diffraction. Au cœur de cette étude, le microscope STEM, doté de sa capacité de résolution nanométrique, joue un rôle central en mesurant l'absorption énergétique à travers la spectroscopie de perte d'énergie des électrons (EELS) transmis. Complétée par un système spectroscopique combiné intégré au microscope, une analyse du spectre de luminescence (cathodoluminescence) des nanostructures a été réalisée.La combinaison de ces techniques a permis de caractériser les excitons dans les matériaux de dimension réduite, notamment des hétérostructures à base de TMDs monocouche (WS2 et MoSe2), préparées au préalable en salle blanche dans le cadre de cette thèse. Les cartographies de luminescence ont révélé des corrélations complexes entre l'intensité d'émission de l'exciton XA et le trion, dépendant des déplacements spatiaux de la sonde sur la surface de l'échantillon. Ces observations ont permis de déduire la dépendance de la génération de trions ou d'excitons en fonction des déformations des couches de l'hétérostructure.L'excitation par une source d'électrons engendre de multiples transitions électroniques, qui, contrairement à une excitation optique, sont difficiles à contrôler. Pour résoudre ce problème, l'équipe STEM au sein du LPS a développé une technique expérimentale, spectroscopie d'excitation en cathodoluminescence (CLE), permettant d'identifier l'électron responsable de l'émission de chaque photon. L'identification de l'électron responsable de l'émission du photon s'est faite par coïncidence temporelle entre l'électron transmis et le photon émis, au moyen d'un photomultiplicateur et d'un détecteur d'électrons résolu temporellement, Timepix3.Une exploration approfondie du détecteur Timepix3, menée au cours de cette thèse, a permis de dévoiler les mécanismes sous-jacents, depuis l'impact initial de l'électron sur la surface du détecteur jusqu'à la détection ultérieure des charges générées par celui-ci au sein de la couche de lecture. Cette étude, basée sur diverses approches expérimentales, a facilité la caractérisation précise du détecteur, contribuant ainsi à l'optimisation de sa résolution temporelle.Cette technique de coïncidence temporelle a été appliquée à d'autres matériaux de faible dimension, notamment aux nanofils d'AlN dotés de puits quantiques de GaN/AlN. Cette approche a permis d'explorer la durée de vie des excitations, révélant une étroite dépendance avec l'écrantage du champ électrique au sein de ces nanofils. Les simulations et les résultats expérimentaux ont révélé des variations notables en fonction du courant et de la position spatiale d'excitation au sein du nanofil. Ces deux dépendances, bien que distinctes, sont étroitement liées dans les effets observés, modulant la migration des charges des barrières vers le puits et exerçant ainsi une influence marquée sur la durée de vie et l'énergie d'émission des excitons.Enfin, une étude énergétique des électrons en coïncidence avec les photons a révélé l'efficacité d'émission pour chaque absorption énergétique, mettant en lumière des processus de désexcitation spécifiques conduisant à la génération d'excitons et à l'émission de photons.Ces résultats ouvrent la voie à de nouvelles perspectives dans le domaine des matériaux de faible dimension pour le développement de dispositifs optoélectroniques, notamment des LEDs
A profound understanding of interactions within luminescent materials under excitation is imperative for advancing optoelectronic devices. Materials with small dimensions exhibit unique optoelectronic properties resulting from quantum effects and spatial confinement.Our approach to analyzing the optoelectronic properties of nanomaterials is marked by a versatile methodology, employing various techniques integrated into the scanning transmission electron microscope (STEM). Utilizing an accelerated electron source at 60 keV, our study successfully overcame diffraction limitations. The STEM microscope, with nanometric resolution capabilities in measuring energy absorption through transmitted electron energy loss spectroscopy (EELS), formed the central aspect of our exploration. Enhanced by an integrated spectroscopic system into the microscope, we performed an in-depth analysis of the luminescence spectrum (cathodoluminescence) of nanostructures.The integration of these techniques facilitates the exploration of optoelectronic effects induced by excitons in low-dimensional materials, particularly in monolayer TMD-based heterostructures (WS2 et MoSe2) that were carefully prepared in a cleanroom. Luminescence mappings revealed correlations between the emission intensity of exciton XA and the trion, depending on the spatial displacements of the probe across the sample surface. These observations enabled deductions about the dependence of trion or exciton generation on the deformations of the layers within the heterostructure.Excitation by an electron source induces multiple electronic transitions, presenting a challenge compared to optical excitation. To tackle this challenge, the STEM team at LPS developed an experimental technique, the cathodoluminescence excitation spectroscopy (CLE), to identify the electron responsible for the emission of each photon. This identification, coupled with the magnetic spectrometer providing information on the energy absorbed by the sample, facilitates identifying the type of excitation leading to photon emission. The identification of the electron responsible for photon emission was achieved through temporal coincidence, utilizing a photomultiplier and a temporally resolved electron detector, Timepix3.A thorough investigation of the Timepix3 detector during this thesis unveiled the underlying mechanisms, spanning from the initial impact of the electron on the detector surface to its subsequent detection within the readout layer. This study, incorporating various experimental approaches, significantly contributed to the precise characterization of the detector, ultimately optimizing its temporal resolution.The temporal coincidence technique was applied to other low-dimensional materials, such as AlN nanowires with GaN/AlN quantum wells. This approach provided insights into the lifetime of excitations, uncovering a close dependence on the screening of the electric field within these nanowires. Simulations and experimental results demonstrated notable variations based on the current and spatial excitation position within the nanowire. While these dependencies are distinct, they are closely interlinked, influencing the migration of charges from barriers to wells and thus exerting a significant impact on the lifetime and emission energy of excitons.Finally, an energy-dependent study of electrons coinciding with photons unveiled the emission efficiency for each energy absorption, highlighting specific de-excitation processes leading to exciton generation, resulting in photon emission.These results not only enhance our comprehension of low-dimensional materials but also forge new pathways for the development of optoelectronic devices, particularly LEDs

Notre travail s'inscrit dans la mise au point de nouveaux circuits intégrées monolithiques de traitement du signal dans la gamme du Ghz. Il porte sur l'étude d'un modulateur acousto-électro-optique formé de multi-puits quantiques ou nous exploitons l'effet du confinement quantique et le phénomène de résonance excitonique. L'absorption optique est modulée par l'effet Stark et les déformations induits par une onde acoustique de surface. Un outil théorique d'optimisation de la structure du modulateur a été mis au point. La méthode des éléments finis est utilisée pour calculer les niveaux énergétiques des bandes de conduction et de valence et les fonctions d'onde électroniques correspondantes tandis que les énergies de liaisons excitoniques sont calculées par la méthode variationnelle. L'influence des différents paramètres sur l'absorption optique est étudiée. L'optimisation donne des résultats très satisfaisants : rapport de contraste de 18db et variation de transmittance de 0,75. Deux prototypes ont été réalisés dans le but de différencier les effets physiques mis en jeu. La caractérisation du composant par photoluminescence et photoréflectance met en évidence la faisabilité du modulateur acousto-electro-optique à puits quantiques et montre la bonne qualité des prototypes réalisés.

Bei der theoretischen Beschreibung von spektroskopischen Experimenten wird in der Regel das Materiesystem quantenmechanisch beschrieben, während das Strahlungsfeld klassisch behandelt wird. Diese semiklassische Näherung ist zur Beschreibung von Experimenten, bei denen eine starke Kopplung zwischen dem Matriesystem und einzelnen Photonen besteht, nicht mehr gültig. Dies kann beispielsweise innerhalb eines optischen Resonators der Fall sein. In dieser Arbeit wird am Beispiel eines Pump-Test- Experiments zum Nachweis des optischen Stark-Effekts untersucht, welche zusätzlichen Effekte sich bei einer quantisierten Beschreibung des Strahlungsfeldes ergeben. Ein signifikanter Effekt ist, dass die Photonenstatistik des Pumpfeldes sich in der Linienform der verschobenen Resonanzlinie widerspiegelt. Weiter wurde in dieser Arbeit bei kleiner Pumpverstimmung ein Verstärkungseffekt gefunden, der ebenfalls auf der quantisierten Behandlung des Strahlungsfeldes beruht (nichtklassische Verstärkung). Es treten ferner bei grosseren Ensemblen von Zwei-Niveau -Systemen zusätzliche Unterstrukturen und Resonanzen auf. Auch kann der Nachweis des optischen Stark-Effekts Aufschluss über die Nichtdiagonalelemente bezüglich der Photonenzahl des quantisierten Pumpfeldes geben.Im Hinblick auf die Beschreibung komplexer Materiesystemen wurde in dieser Arbeit auch eine näherungsweise Berechnung der Testabsorption mit quantisiertem Strahlungsfeld im Rahmen einer Dichtematrixtheorie untersucht. Insbesondere war hier für die quantitative Beschreibung der nichtklassischen Verstärkung eine Berücksichtigung hoherer Korrelationen zwingend erforderlich. Auch wurden näherungsweise Entkopp- lungen unter Berücksichtigung der Erhaltungsgrossen durch- geführt. Die Dichtematrixtheorie wurde auf die Untersuchung des optischen Stark-Effektes an storstellengebundenen Exzitonen in Halbleitern angewandt. Da diese Resonanzen vergleichsweise kleine homogene und inhomogene Linienbreiten aufweisen,ist hier experimentell zu erwarten, dass sich feine Effekte des quantisierten Pumpfeldes bemerkbar machen konnen.
The theoretical description of spectroscopic experiments usu ally relies on a semiclassical approach where the matter system is described in terms of quantum mechanics while the radiation field is treated classically. This approach does n ot work well for systems with a strong coupling between the matter system and photons of the radiation field. The latter can be the case within an optical resonator.In this thesis, additional effects of a quantized radiation field are inves tigated on a pump-probe experiment for detecting the optical Stark effect. One significant effect is that the lineshape of the shifted resonance displays the photon statistics of the pump field. For small pump detuning probe gain results in a frequency regime where the semiclassical treatment predicts absorption. This effect is refered to nonclassical gain. For larger ensembles of two-level systems, additional substructures and resonances appear within the probe absorption spectrum. Also non- diagonal elements of the field density matrix can be detected in such an experiment. In order to describe a more complex matter systems, the optical Stark effect has been treated in terms of a density matrix approach with quantized radiation fields. For a quantitative description of nonclassical gain, higher correlation terms had to be treated properly. Moreover, conserved quantities were taken into account in approximate decouplings. The density matrix approach was applied to the description of the optical Stark effect on impurity-bound excitons in semiconductors. These systems are of high interest as their narrow resonances might allow the demonstration of fine effects of the quantized radiation field.

Designs for deep ultraviolet (DUV) edge emitting laser diodes (LDs) based on the wurtzite III-nitride (III-N) material system are presented. A combination of proprietary and commercial advanced semiconductor LD simulation software is used to study the operation of III-N based DUV LDs theoretically. Critical factors limiting device performance are identified based on an extensive literature survey. A comprehensive design parameter space is investigated thoroughly with the help of advanced scripting capabilities. Several design strategies are proposed to eliminate the critical problems completely or partially. A DUV LD design is proposed based exclusively on AlInN active layers grown epitaxially on bulk AlN substrates because AlInN offers a promising alternative to AlGaN for the realization of LDs and LEDs operating in the DUV regime. The proposed AlInN-based design also features a tapered electron blocking layer (EBL) instead of a homogeneous one. Tapered EBLs redistribute the interfacial polarization charge volumetrically throughout the entire EBL thickness via compositional grading, and eliminate the parasitic inversion layer charge. AlGaN based DUV LD designs are explored also because at present, it may be difficult to grow AlInN epitaxially with superior crystalline quality. Polarization charge matching is proposed to improve electron and hole wavefunction overlap within the active region. Although the strategy of polarization charge matching has already been proposed in the literature to enhance performance of visible wavelength LEDs and LDs, the proposed design presents the first demonstration that polarization charge matching is also feasible for DUV LDs operating at sub-300 nm wavelengths. A lateral current injection (LCI) LD design is proposed featuring polarization-charge-matched barriers and regrown Ohmic contacts to avoid a group of issues related to the highly inefficient p-type doping of wide bandgap III-N materials in vertical injection designs. The proposed design partially decouples the problem of electrical injection from that of optical confinement. Although the idea of an LCI LD design has been proposed in the literature in the 90s to be used as longer wavelength active sources in optoelectronic integrated circuits using GaInAsP/InP and related material systems, the proposed design is the first theoretical demonstration that this concept can be applied to DUV LDs based on III-N material system. To solve the problem of hole transport in vertical injection designs, a DUV LD design based exclusively on AlGaN material system is presented, featuring an inverse-tapered p-waveguide layer instead of an EBL. Several EBL designs are investigated, and compared with conventionally-tapered EBL design. Through judicious volumetric redistribution of fixed negative polarization charge, inverse tapering may be exploited to achieve nearly flat valence band profiles free from barriers to hole injection into the active region, in contrast to conventional designs. Numerical simulations demonstrate that the inverse tapered strategy is a viable solution for efficient hole injection in vertical injection DUV LDs operating at shorter wavelengths (< 290 nm).

Despite enormous efforts and investments, the efficiency of InGaN-based green and yellow-green light emitters remains relatively low, and that limits progress in developing full color display, laser diodes, and bright light sources for general lighting. The low efficiency of light emitting devices in the green-to-yellow spectral range, also known as the “Green Gap”, is considered a global concern in the LED industry. The polar c-plane orientation of GaN, which is the mainstay in the LED industry, suffers from polarization-induced separation of electrons and hole wavefunctions (also known as the “quantum confined Stark effect”) and low indium incorporation efficiency that are the two main factors that contribute to the Green Gap phenomenon. One possible approach that holds promise for a new generation of green and yellow light emitting devices with higher efficiency is the deployment of nonpolar and semi-polar crystallographic orientations of GaN to eliminate or mitigate polarization fields. In theory, the use of other GaN planes for light emitters could also enhance the efficiency of indium incorporation compared to c-plane. In this thesis, I present a systematic exploration of the suitable GaN orientation for future lighting technologies. First, in order to lay the groundwork for further studies, it is important to discuss the analysis of processes limiting LED efficiency and some novel designs of active regions to overcome these limitations. Afterwards, the choice of nonpolar orientations as an alternative is discussed. For nonpolar orientation, the (1-100)-oriented (m-plane) structures on patterned Si (112) and freestanding m-GaN are studied. The semi-polar orientations having substantially reduced polarization field are found to be more promising for light-emitting diodes (LEDs) owing to high indium incorporation efficiency predicted by theoretical studies. Thus, the semi-polar orientations are given close attention as alternatives for future LED technology. One of the obstacles impeding the development of this technology is the lack of suitable substrates for high quality materials having semi-polar and nonpolar orientations. Even though the growth of free-standing GaN substrates (homoepitaxy) could produce material of reasonable quality, the native nonpolar and semi-polar substrates are very expensive and small in size. On the other hand, GaN growth of semi-polar and nonpolar orientations on inexpensive, large-size foreign substrates (heteroepitaxy), including silicon (Si) and sapphire (Al2O3), usually leads to high density of extended defects (dislocations and stacking faults). Therefore, it is imperative to explore approaches that allow the reduction of defect density in the semi-polar GaN layers grown on foreign substrates. In the presented work, I develop a cost-effective preparation technique of high performance light emitting structures (GaN-on-Si, and GaN-on-Sapphire technologies). Based on theoretical calculations predicting the maximum indium incorporation efficiency at θ ~ 62º (θ being the tilt angle of the orientation with respect to c-plane), I investigate (11-22) and (1-101) semi-polar orientations featured by θ = 58º and θ = 62º, respectively, as promising candidates for green emitters. The (11-22)-oriented GaN layers are grown on planar m-plane sapphire, while the semi-polar (1-101) GaN are grown on patterned Si (001). The in-situ epitaxial lateral overgrowth techniques using SiNx nanoporous interlayers are utilized to improve the crystal quality of the layers. The data indicates the improvement of photoluminescence intensity by a factor of 5, as well as the improvement carrier lifetime by up to 85% by employing the in-situ ELO technique. The electronic and optoelectronic properties of these nonpolar and semi-polar planes include excitonic recombination dynamics, optical anisotropy, exciton localization, indium incorporation efficiency, defect-related optical activities, and some challenges associated with these new technologies are discussed. A polarized emission from GaN quantum wells (with a degree of polarization close to 58%) with low non-radiative components is demonstrated for semi-polar (1-101) structure grown on patterned Si (001). We also demonstrated that indium incorporation efficiency is around 20% higher for the semi-polar (11-22) InGaN quantum wells compared to its c-plane counterpart. The spatially resolved cathodoluminescence spectroscopy demonstrates the uniform distribution of indium in the growth plane. The uniformity of indium is also supported by the relatively low exciton localization energy of Eloc = 7meV at 15 K for these semi-polar (11-22) InGaN quantum wells compared to several other literature reports on c-plane. The excitons are observed to undergo radiative recombination in the quantum wells in basal-plane stacking faults at room temperature. The wurtzite/zincblende electronic band-alignment of BSFs is proven to be of type II using the time-resolved differential transmission (TRDT) method. The knowledge of band alignment and degree of carrier localization in BSFs are extremely important for evaluating their effects on device properties. Future research for better understanding and potential developments of the semi-polar LEDs is pointed out at the end.

In der vorliegenden Arbeit wird das Hauptaugenmerk auf die Untersuchung der Auswirkungen einer Modifikation der zugänglichen Prozessparameter auf die funktionalen Eigenschaften oxidischer Dünnfilme während der gepulsten Laserabscheidung (PLD) gelegt. Der erste Teil der Arbeit stellt die Herstellung von BaTiO3/SrTiO3-Mehrfach-Heterostrukturen auf thermisch und chemisch vorbehandelten SrTiO3-Substraten mittels gepulster Laserabscheidung (PLD) vor. Die zugängliche in-situ Wachstumskontrolle durch ein reflection high-energy electron diffraction (RHEED)-System ermöglicht es die Wachstumsprozesse in Echtzeit zu überwachen. Angestrebt wird ein stabiler zwei-dimensionaler Wachstumsmodus, der neben glatten Grenzflächen auch eine hohe Dünnfilmqualität ermöglicht. Es wird erstmals die prinzipielle Anwendbarkeit von BaTiO3/SrTiO3-Heterostrukturen als Bragg-Spiegel aufgezeigt. Für BaTiO3- sowie SrTiO3-Dünnfilme wurden die PLD-Parameter Substrattemperatur, Sauerstoffpartialdruck, Energiedichte des Lasers sowie Flussdichte der Teilchen variiert und die Auswirkungen auf die strukturellen, optischen und Oberflächeneigenschaften mittels Röntgendiffraktometrie (XRD), spektraler Ellipsometrie (SE) und Rasterkraftmikroskopie (AFM) beleuchtet. Im zweiten Teil werden ZnO/MgxZn1−xO-Quantengrabenstrukturen hetero- und homoepitaktisch auf thermisch vorbehandelten a-Saphir- respektive m- und a-orientierten ZnO-Einkristallen vorgestellt. Die Realisierung eines zwei-dimensionalen „layer-by-layer“ Wachstumsmodus wird für die Quantengrabenstrukturen aufgezeigt. Die Quantengrabenbreite lässt sich aus beobachteten RHEED-Oszillationen exakt bestimmen. Ein Vergleich zwischen, mittels Photolumineszenz gemessenen Quantengrabenübergangsenergien als Funktion der Grabenbreite mit theoretisch ermittelten Werten wird vorgestellt, wobei der Unterschied zwischen polaren und nicht-polaren Strukturen mit Blick auf eine Anwendung aufgezeigt wird. Für c-orientierte ZnO-Dünnfilme wird das Wachstum im Detail untersucht und ein alternativer Abscheideprozess im so genannten Intervall PLD-Verfahren vorgestellt. Die Verifizierung der theoretischen Prognose einer ferromagnetischen Ordnung mit einer Curie-Temperatur oberhalb Raumtemperatur (RT) für kubische, Mangan stabilisierte Zirkondioxid (MnSZ)-Dünnfilme stellt den dritten Teil der Arbeit dar. Die strukturellen Eigenschaften der Dünnfilme werden mittels XRD, AFM sowie Transmissionselektronenmikroskopie (TEM) untersucht. Die Bedingungen einer erfolgreichen Stabilisierung der kubischen Kristallphase durch den Einbau von Mn wird aufgezeigt. Mittels Röntgenphotoelektronenspektroskopie (XPS) sowie Elektronenspinresonanz (EPR) wird der Ladungszustand der, in der Zirkondioxidmatrix eingebauten, Mn-Ionen ermittelt. Die elektrischen Eigenschaftenwerden durch Strom-Spannungsmessungen(IU) sowie der Leitungstyp durch Seebeck-Effekt Messungen charakterisiert. Zur Erhöhung der Leitfähigkeit werden die MnSZ Dünnfilme in verschiedenen Atmosphären thermisch behandelt und Veränderungen durch IU-Messungen aufgezeigt. Ergebnisse von optischen Untersuchungen mittels Transmissionsmessungen und KL werden präsentiert. Superconducting quantum interference device (SQUID)-Magnetometrie wird zur Charakterisierung der magnetischen Eigenschaften genutzt. Magnetische Ordnungen im Bereich zwischen 5 K ≤ T ≤ 300 K werden untersucht und der Einfluss von Defekten sowie einer thermischen Behandlung in verschiedenen Atmosphären auf die magnetischen Eigenschaften diskutiert.

L'application des résonances de Förster à plusieurs corps est étudiée pour réaliser des circuits de portes quantiques multi-qbits. Deux nouveaux types de transitions borroméennes à trois atomes utilisant un atome relais ont été proposées et étudiées numériquement. En particulier, une résonance de Förster à trois atomes non isolée et contrôlée par effet Stark entre des états S et P de niveaux élevés n = 80, 81, 82 avec des atomes de Rb isolés dans des pièges optiques a été modélisée. Une résonance de Förster isolée à trois atomes a également été démontrée pour les états n = 70, 71 des atomes Rb. Les résonances ont été étudiées dans une configuration spatiale fixe, ce qui nous a permis de démontrer l'évolution cohérente de la population et de la phase des états collectifs impliqués. Des schémas de portes de Toffoli à trois qubits ont été développés et modélisés numériquement sur la base des résonances démontrées dans des ensembles à trois atomes. En outre, un schéma généralisé de porte de phase doublement contrôlée CCPHASE a été développé sur la base de la résonance de Förster à trois corps induite par radiofréquence. De plus, un schéma de porte quantique similaire a été proposé sur la base de la résonance de Förster induite par radiofréquence à deux atomes avec un déplacement contrôlé par interaction avec le troisième. Les performances rapides et la grande fidélité des schémas proposés, ainsi que leur robustesse potentielle aux erreurs, nous permettent d'espérer le succès d'une réalisation expérimentale prochainement
Application of few-body Förster resonances for implementation of multiqubit quantum gate circuits has been investigated. New types of three-atom Borromean transitions based on the relay atom have been proposed and numerically studied. In particular, a Stark-controlled non-isolated three-atom Förster resonance between high-lying n = 80, 81, 82 S − P states of Rb atoms isolated in individual optical traps has been modeled. Isolated three-atom Förster resonance has also been demonstrated for n = 70, 71 states of Rb atoms. The resonances were investigated in a fixed spatial configuration, allowing us to demonstrate the coherent population and phase dynamics of the collective states involved. Three-qubit Toffoli gates schemes have been developed and numerically modeled based on the demonstrated resonances. Also, a generalized doubly controlled phase CCPHASE gate scheme has been developed based on the radiofrequency-induced three-body Förster resonance. Additionally, a similar quantum gate scheme has been proposed based on two-atom RF-induced Förster resonance with controlled displacement. The fast performance and high fidelity of the proposed schemes, as well as their potential robustness to errors, allow us to expect a successful experimental implementation in the near future

In this work we establish and test the technique of parallel adiabatic passage (PLAP) thatoptimizes the adiabatic passage in the sense that it selects specific paths that allow a fastadiabatic dynamics while preserving the standard robustness of adiabatic techniques. Theintuition of PLAP is based on the fact that the use of eigenvalues that are parallel for alltimes is expected to lead to a small nonadiabatic transition probability from Landau-Zeneranalysis for two-state approximations. In this work we test the robustness of this techniqueand show its superiority to the traditional linearly chirped dynamics with Gaussian pulses. Weshow its extension for two-photon and three-photon transitions on multilevel quantum systems,where the Stark shift plays an important role in a strong field regime. We have determined anoptimal pulse shaping in which the static and dynamic energy level shifts are simultaneouslycompensated by a programmed phase of a laser field. Next the local parallel adiabatic passagetechnique is presented. This corresponds to a dynamics where the eigenvalue of the populatedstate is parallel to the closest one at all times.We extend the idea of population transfer by adiabatic passage from the ground state toa superposition of states. The transfer is executed with spectrally shaped femtosecond laserpulses. The excited states are dynamically shifted in energy due to the presence of nonresonantcomponents of different channels. We show that this Stark shift can be compensated by anotherfield or by shaping appropriately the pulses.

Aujourd’hui les interconnections optiques ont devancé les interconnections électriques à longue, moyenne et courte distance dans le domaine des télécommunications. La photonique silicium a connu un tel développement que même les interconnections inter et intra puces deviennent progressivement à dominante optique. En revanche, la multiplication des terminaux d’accès et l’augmentation constante du volume de données échangées imposent l’apparition de nouveaux composants avec une consommation énergétique encore plus faible. Dans ce contexte, les composants optoélectroniques à faible consommation à base des puits quantiques Ge/SiGe ont été développés. Jusqu’à présent l’utilisation des puits quantiques Ge/SiGe était seulement limitée aux modulateurs à électro-absorption Les travaux menés durant la première partie de ma thèse consistaient à étudier un nouveau type de région active à base de puits quantiques Ge/SiGe couplés. Ces études ont abouti à la démonstration d’un effet d’électro-réfraction géant dans ces structures. La région active basée sur les puits couplés donne lieu à une variation de l’indice de réfraction de 2.3×10-3 sous une tension de 1.5 V seulement. L’utilisation d’un tel effet pour la réalisation de modulateurs optiques intégrés a ensuite nécessité le développement des briques de base passives afin d’obtenir une structure interférométrique. Des virages compacts et des interféromètres de Mach Zehnder sont conçus, fabriqués et caractérisés avec succès. La sensibilité de ces structures à la polarisation est évaluée par simulation numérique et les structures insensibles à la polarisation sont conçues. Un modulateur à électroréfraction intégré est ensuite conçu et fabriqué, nécessitant la mise en place d’un nouveau procédé technologique. Les résultats de caractérisation préliminaires sont présentés. Les perspectives de ce travail sont la réalisation d’un modulateur efficace ayant une tension de commande inférieure à 2V.Le champ d’application des circuits photoniques ne se limite pas au secteur des télécommunications. L’approche basée sur l’optique intégrée est aussi très prometteuse pour l’identification et analyse des espèces chimiques environnantes. La région spectrale de moyen infrarouge est particulièrement adaptée à cet effet car les raies d’absorption spécifiques de nombreuses espèces chimiques y sont présentes. L’utilisation des circuits optiques sur substrat silicium permet de développer des systèmes spectroscopiques performants, compacts et à bas cout. La seconde partie de ma thèse était dédiée au développement de la plateforme photonique large-bande basée sur les guides d’ondes Si1-xGex riches en Ge. Les guides d’onde large bande fonctionnant entre 5.5 et 8.6 µm ont été démontrés expérimentalement ce qui a permis de concevoir des structures plus complexes telles que les MMI et les interféromètres de Mach Zehnder ultra large bande. Le même dispositif possède une bande passante théorique de 3.5 µm en polarisation TE et d’une octave en polarisation TM. Le fonctionnement a été démontré expérimentalement entre 5.5 et 8.6 µm et est seulement limité par la plage de longueurs d’ondes adressable par le laser. Ce travail ouvre les perspectives pour la future démonstration des systèmes spectroscopiques ultra-large bande sur la plateforme Si1-xGex riche en Ge. Une dernière partie de ce travail a été consacrée à l’étude de la génération de la seconde harmonique dans les puits quantiques Ge/SiGe pour les systèmes spectroscopiques dans le moyen infrarouge. Les premières structures sont conçues et fabriquées
Today optical interconnects have overpassed wires on long, mid and short distances on the telecommunication field. Silicon photonics have known such a development that even inter and intra chip communications progressively become optical. However, the multiplication of data access terminals and the constant increase of data consumption force new components with even lower power consumption to appear. In this context, low power consumption components based on Ge/SiGe quantum wells have been developed. Until now, the use of Ge/SiGe quantum wells has been only limited to electroabsorption modulators. The first part of my thesis was dedicated to the study of a new kind of active region based on coupled Ge/SiGe quantum wells. This work led to the demonstration of giant electrorefractive effect in these structures. The active region based on coupled quantum wells gives a refractive index variation of 2.3×10-3 under a bias of only 1.5 V. The use of this effect for the development of integrated optical modulators needed the development of main building blocks to obtain interferometric structures. Compact bends and Mach Zehnder interferometers have been designed, fabricated and successfully characterized. The sensitivity to the polarization of these structures was evaluated with numerical simulations and polarization insensitive structures were designed. Then, an integrated electrorefractive modulator has been designed and fabricated which needed the development of a new technological process. The first charaterization results are presented. The perspectives of this work are the realization of an efficient modulator with switching voltage lower than 2V. The field of application of photonic integrated circuits is not only limited to the telecommunications. The approach based on integrated optics is also very promising for the identification and analysis of surrounding chemical species. Mid infrared spectral region is particularly suitable for this purpose as it contains specific absorption fingerprints of different chemical species. The use of photonic integrated circuits on silicon substrate allows to develop performant, compact and low cost spectroscopic systems. The second part of my thesis was focused on the development of wideband photonic platform based on Ge-rich Si1-xGex waveguides. Wideband waveguides between 5.5 and 8.5 µm were experimentally demonstrated which made possible the developpement of more complex structures such as MMIs or ultra-wideband Mach Zehnder interferometers. The same device has a theoretical bandwidth of 3.5 µm in TE polarization and of one octave in TM polarization. The operation was experimentally demonstrated between 5.5 and 8.6 µm and is only limited by laser spectral range. This work paves the way for future development of ultra-wideband spectroscopic systems on Ge-rich Si1-xGex platform. The last part of this work concerned second harmonic generation in Ge/SiGe quantum wells for mid infrared spectroscopic systems. First test devices have been designed and fabricated

Die Arbeit befaßt sich mit der Messung und Analyse der spezifischen Wärme verschiedener stark korrelierter Elektronensysteme bei tiefen Temperaturen und hohen Magnetfeldern. Zunächst wird der im Rahmen dieser Arbeit verwendete, auf der Meßmethode der thermischen Relaxation beruhende Aufbau des Kalorimeters (Einsatzbereich 0.05K&lt;T&lt;4K und 0&lt;B&lt;12T) ausführlich erläutert. Danach werden die Ergebnisse von Messungen an den drei Schwere-Fermionen-Verbindungen CeCu2Si2, CeNi2Ge2 und YbRh2Si2 dargelegt. Wenngleich alle drei Systeme bei tiefen Temperaturen durch den für Schwere-Fermionen-Systeme charakteristischen, stark erhöhten elektronischen Beitrag zur spezifischen Wärme gekennzeichnet sind zeigen sich deutliche Unterschiede im beobachteten Grundzustandsverhalten. An CeCu2Si2 wird die für T&lt;1K auftretende Konkurrenz zwischen einem supraleitenden und einem magnetischen Grundzustand ausführlich studiert. In YbRh2Si2 zeigt sich bei einer für 4f-Systeme bemerkenswert tiefen Temperatur von ca. 70mK ein Übergang in eine magnetische Phase, während der Grundzustand von CeNi2Ge2 wegen stark ausgeprägter Probenabhängigkeiten immer noch kontrovers diskutiert wird. Des weiteren zeigen alle drei Verbindungen deutliche Abweichungen vom Verhalten einer Fermi-Flüssigkeit. Die Theorie der Fermi-Flüssigkeit hat sich für metallische Verbindungen als sehr erfolgreich auch bei der Beschreibung des Verhaltens eines Systems aus stark wechselwirkenden Ladungsträgern erwiesen. Warum diese Theorie auf die untersuchten Verbindungen nicht anwendbar zu sein scheint, wird im Rahmen moderner Modellvorstellungen wie z. B. der Nähe zu einem quantenkritischen Punkt diskutiert. Die an Sr2RuO4, dem ersten Kupfer-freien Perowskit Supraleiter, durchgeführten Messungen der spezifischen Wärme dokumentieren das Auftreten von zwei Zusatzbeiträgen für T&lt;Tc, die eine Interpretation der spezifischen Wärme des supraleitenden Zustands von Sr2RuO4 im Hinblick auf die Topologie des Ordnungsparameters deutlich erschweren.

碩士
國立成功大學
電機工程研究所
80
The purpose of this thesis is to investigate the mechanism of the quantum well self-electro-optic effect device (SEED): Quantum confined Stark effect and the theory of binding exciton in a quantum well will be dicussed. First, according to the one-dimension time-independence Schrodinger equation, the discrete energy levels and the wave function in the quantum wells are calculated by a new numerical analysis method. 　　Second, a variational method with separable trial funtion is employed to evaluate the binding energy of an exciton in a quantum well. Then,the position of the exciton absorption peads with applied field perpendicular to quantum-well layers can be predicted. Finally, considering the theoretical model of exciton spectrum, the integrated intensity of the optical absorption spectrum of ground-state electron-heavy-hole exciton resonance both in III-V and II-VI semiconductor quantum wells are calculated. It is found that II-VI quantum-wells have higher room-temperature excitonic saturation. 　　The optimal device parameters of the SEEDs can be then determined.

Cette thèse de doctorat concerne deux problèmes mathématiques issus de la mécanique quantique. On considère une particule quantique, non relativiste et sans spin, astreinte à se mouvoir sur une surface bidimensionnelle $\cal S$, plongée dans un champ magnétique homogène qui lui est perpendiculaire. Dans un premier problème, $(\cal S)=\R\times \mathbb(S)_L^1$, qui est un cylindre infini de circonférence $L$, ce qui correspond à des conditions aux bords periodiques. Dans le deuxième cas, $(\cal S)=\R^2$. En fonction du problème étudié, on ajoute un potentiel convenable. On est ainsi amené à étudier deux opérateurs de Schrödinger. Le premier opérateur analysé génère la dynamique d'une particule soumise à un potentiel aléatoire de type Anderson ainsi qu'un potentiel non aléatoire dont le but est de confiner la particule le long de l'axe du cylindre, sur une longueur $L$. Dans ce cas, on localise le spectre et on le classifie par le courant quantique porté par les fonctions propres correspondantes. On montre qu'il y a des régions spectrales où n'existent que des valeurs propres avec courant d'ordre un par rapport à $L$, et des régions spectrales où sont mélangées valeurs propres avec courant d'ordre un et valeurs propres avec courant infinitésimal par rapport à $L$. Ces resultats on un intétet physique dans le cadre de l'effect Hall entier. Le deuxième opérateur de Schrödinger étudié, correspond à la situation physique où le potentiel est donné par la somme d'un potentiel ``local'' et d'un potentiel dû à un petit champ électrique $F$ constant. Dans ce cas on montre que les états résonants induits par le champ électrique décroissent exponentiellement avec un taux donné par la partie imaginaire des valeurs propres d'un certain opérateur non auto-adjoint. On montre de plus que cette partie imaginaire possède une borne supérieure de l'ordre de $\exp(-1/F^2)$, pour $F$ tendant vers zéro. Ainsi, le temps de vie de l'état résonant en question est au moins de l'ordre de $\exp(1/F^2)$.

碩士
國立臺灣大學
電子工程學研究所
96
Optical communications have dominated the intermediate to long distance data transmission and also gradually replaced the metal interconnects for the short-distance links. The decreasing device size in silicon chips increases the interconnect resistance and hence degrades the system speed severely, thus the optical interconnects is one of the solutions to enable high-speed and high-capacity chip-scale communication technology. The high-speed external optical modulator is one of the key components routinely used in today’s optical communications. The Quantum confined stark effect (QCSE) – one of the most effective modulator operating theorems – can enable high-speed external modulation with low operation voltage. The QCSE had been demonstrated in the germanium quantum well system grown on silicon and would enable optical interconnects integrated with silicon chips. The QCSE at room temperature with thick quantum well was investigated in this thesis study. Since both silicon and germanium are indirect bandgap materials, there exist not only direct gap absorption transition but also indirect gap absorption with lower transition energy which leads to the background absorption. An electro-absorption measurement system was setup to study the QCSE as well as the direct and indirect absorption. The thick quantum well structure exhibits electroabsorption effect in the C-band and has lower quantum well energy, weaker exciton, and less indirect absorption. Besides, the simulations based on the tunneling resonance method are discussed.

In this thesis we present a study about strong light-matter interaction in a broad single GaAs/AlGaAs quantum well representing a 3-level system. In particular we investigate the AC-Stark effect, where we observe in THz absorption spectra an Autler-Townes splitting as well as a Mollow-triplet. Compared to previous work, we showed for the first time an all-THz pump-probe experiment in the THz regime below the Reststrahlenband. Furthermore, we observe a strong frequency shift in the absorption energy of the first intersubband transition depending on the charge carrier density in the quantum well. The Autler-Townes splitting as well as the absorption frequency shift can be potentially exploited for THz-modulation applications. Beyond nonlinear optics many interesting effects occur in the strong light-matter interaction regime such as Rabi oscillations, coherent population trapping, lasing without inversion, electromagnetically induced transparency (EIT) and the AC-Stark effect. Our quantum well represents a 3-level system in which we investigate a splitting behaviour in the absorption spectrum of the first and second intersubband transition. Especially a splitting for the first intersubband transition is predicted also for electromagnetically induced transparency, while the second intersubband transition is pumped with a strong varying electric field. Naturally, a fundamental question is, how to distinguish EIT and an Autler-Townes duplet since both result in a spectrally transparent window. The method of choice for investigations combines narrowband pulses in the THz range provided by a free-electron laser and broadband THz pulses generated in a GaP crystl within a THz time-domain spectroscopy setup. In this unique configuration we perform time-resolved pump and probe spectroscopy experiments by pumping resonantly the second intersubband transition at 3.4 THz to induce a splitting of the second and third subband. Broadband THz pulses then probe an absorption splitting of about 0.2 THz related to the first intersubband transition at ≈ 2.3 THz as well as a splitting of the second intersubband transition (Mollow triplet). Analyzing experiments and using a theoretical criteria to distinguish EIT and Autler-Townes splitting, we conclude to observe an Autler-Townes doublet instead of an EIT effect.
In dieser Arbeit berichten wir über die starke Licht-Materie Wechselwirkung in 3-Niveau system anhand eines einzelnen, breiten GaAs/AlGaAs Quantentopfes. Insbesondere untersuchen wir den AC-Stark Effekt und beobachten eine Aufspaltung des Absorptionsspektrums durch das Autler-Townes Dublett und das Mollow Triplett. Im direkten Vergleich mit vorangegangenen Arbeiten zeigen wir zum ersten Mal ein reines THz Anrege-Abfrage Experiment mit Frequenzen unterhalb des Reststrahlenbandes. Weiterhin beobachten wir eine starke Frequenzverschiebung der Absorptionsenergie des ersten Intersubbandübergangs in Abhängigkeit von der Ladungsträgerdichte im Quantentopf. Sowohl das Autler-Townes Dublett als auch die Verschiebung der Absorptionsfrequenz ermöglichen potentielle Anwendung im Bereich der THz-Modulation. Im Bereich der starken Licht-Materie Wechselwirkung sind viele interessante Effekte beobachtbar wie Rabi Oszillationen, coherent population trapping, Lasern ohne Inversion, elektromagnetisch induzierte Transparenz (EIT) und der AC-Stark Effekt. Unser Quantentopf stellt ein 3-Niveau System dar, in welchem wir eine Aufspaltung der Absorption bezüglich des ersten und zweiten Intersubbandübergangs beobachten. Insbesondere für den ersten Intersubbandübergang ist auch eine Absorptionsaufspaltung durch den EIT Effekt vorhergesagt, während der zweite Intersubbandübergang durch ein starkes, elektrisches Wechselfeld angeregt wird. Es stellt sich dann die Frage, wodurch sich die Effekte EIT und Autler-Townes splitting unterscheiden, weil beide durch ein spektrales transparentes Fenster gekennzeichnet sind. Die von uns gewählte Methode verknüpft schmalbandige, starke elecktrische Wechselfelder im THz-Bereich eines freien Elektronen Lasers und breitbandigen THz-Pulsen, welche durch nichtlineare optische Effekte in einem THz Zeit-Bereichs Spektroskopie Aufbaus erzeugt werden. In dieser einzigartigen Konfiguration führen wir zeitaufgelöste Anrege-Abfrage Spektroskopie Experimente durch, in dem wir den zweiten Intersubbandübergang bei 3, 4 THz nahezu resonant anregen und das zweite und dritte Subband aufspalten. Mit breitbandigen THz Pulsen fragen wir dann die Absorptionsaufspaltung von ca. 0, 2 THz des ersten Intersubbandübergangs bei ≈ 2, 3 THz und des zweiten Intersubbandübergangs (Mollow-Triplett) ab. Nach Auswerten der Experimente und theoretischer Kriterien für die Unterscheidung zwischen EIT und Autler-Townes splitting schlussfolgern wir, ein Autler-Townes Dublett zu beobachten.

碩士
國立臺灣大學
電子工程學研究所
103
GaN-based light-emitting diodes (LEDs) are typically grown on c-plane sapphire, or even patterned sapphire substrates (PSSs). In the same growth condition, we adopt wet etching to fabricate our PSSs with structure depth about 0.5µm instead of dry etching with depth up to 1.6µm. However, we find that the quantum-confined Stark effect (QCSE) can be reduced by changing the geometry of PSSs. Moreover, we have found a probable key parameter which dominates the QCSE magnitude, so that we can predict a probable range to further minimize the QCSE. In the device level, we demonstrate that by reducing QCSE, the optical performance of LED devices such as internal quantum efficiency (IQE) and external quantum efficiency (EQE) can be enhanced, but efficiency droop is larger. After our analysis through the differential of EQE, the efficiency droop should be attributed to the consequence of increasing IQE. In the end, in comparison to the LED devices grown on conventional PSSs, our light output power (LOP) and EQE can reach up to 95% of the conventional one. Therefore, the reduction of QCSE is effective to enhance the performance of LEDs, and it’s potential to be an alternative to fabricate LEDs without changing the crystal growth conditions.

abstract: This dissertation aims to study and understand relevant issues related to the electronic, spin and valley transport in two-dimensional Dirac systems for different given physical settings. In summary, four key findings are achieved. First, studying persistent currents in confined chaotic Dirac fermion systems with a ring geometry and an applied Aharonov-Bohm flux, unusual whispering-gallery modes with edge-dependent currents and spin polarization are identified. They can survive for highly asymmetric rings that host fully developed classical chaos. By sustaining robust persistent currents, these modes can be utilized to form a robust relativistic quantum two-level system. Second, the quantized topological edge states in confined massive Dirac fermion systems exhibiting a remarkable reverse Stark effect in response to an applied electric field, and an electrically or optically controllable spin switching behavior are uncovered. Third, novel wave scattering and transport in Dirac-like pseudospin-1 systems are reported. (a), for small scatterer size, a surprising revival resonant scattering with a peculiar boundary trapping by forming unusual vortices is uncovered. Intriguingly, it can persist in arbitrarily weak scatterer strength regime, which underlies a superscattering behavior beyond the conventional scenario. (b), for larger size, a perfect caustic phenomenon arises as a manifestation of the super-Klein tunneling effect. (c), in the far-field, an unexpected isotropic transport emerges at low energies. Fourth, a geometric valley Hall effect (gVHE) originated from fractional singular Berry flux is revealed. It is shown that gVHE possesses a nonlinear dependence on the Berry flux with asymmetrical resonance features and can be considerably enhanced by electrically controllable resonant valley skew scattering. With the gVHE, efficient valley filtering can arise and these phenomena are robust against thermal fluctuations and disorder averaging.
Dissertation/Thesis
Doctoral Dissertation Electrical Engineering 2017

Theoretical investigation of the dynamics of adiabatic quantum mechanics in two different, highly polar systems has been made. The systems were chosen for their fundamental scientific interest, as they represent atoms and molecules with exaggerated properties, as well as ease of experimental study as such highly polar systems are easier to manipulate using readily-available electric fields. A model two-level system is used to derive one approach for maximizing the probability of adiabatic passage through an avoided crossing and this is compared with the classic Landau-Zener result, and the commonly encountered spin-flip problem of a particle with spin located in a rotating magnetic field. This approach is applied to the avoided crossing between the n = 13, n1 − n2 = 11 (dipole moment of 532 D) and the n = 14, n1 − n2 = −12 (dipole moment of -657 D) highly polar Stark states of the lithium atom at 447 kV/m. Ion-pair formation from two neutral lithium atoms, one in the 2s ground state and the other in an excited state, is also investigated. The cross section σ(v) for free ion-pairs is calculated for the initial colliding pairs of atomic states located below the ion-pair threshold. Li(2s) + Li(3d) is seen to possess the largest cross section (σ(v0) = 569.2 a.u.) at its threshold velocity. The implications of this for bound ion-pair, i.e. heavy Rydberg system, production are briefly discussed. Furthermore, experimental progress towards the production of these atomic and molecular systems from a beam of lithium is presented.
Thesis (Master, Physics, Engineering Physics and Astronomy) -- Queen's University, 2009-12-09 16:49:41.184

碩士
國立交通大學
電子物理系所
99
This thesis theoretically investigates the electronic structures and optical properties of InAs/GaAs self-assembled quantum dots under external electric fields by using six-band Luttinger-Kohn k?況 theory. First, the single-particle (conduction electron or valence hole) spectra of box, pyramid, and truncated-pyramid shaped quantum dots are calculated by using finite difference method. The strain distributions in and out of dots are computed by using finite element software package Comsol multiphysics®. Based on the single particle spectra, optical polarization degree of the ground states of an exciton photo-generated in a quantum dot is calculated by using Fermi’s golden rule. The strain calculations show that the effective confining potential for heavy-hole in a strained dot is governed by out-of-plane strain while the one for light-hole by in-plane strain. The theoretical results show that, compared with box and truncated-pyramid shaped dots, heavy- and light-hole coupling is significantly increased in a pyramid-shaped dot because of larger hydrostatic strain (smaller bi-axial strain) in the narrow upper region of the nano-pyramid. With more light-hole component, larger optical polarization degree is observed for high pyramid-shped dots. Furthermore, the light-hole component in a hole ground state can be significantly changed by applying an external electric field along the growth-axis. As a result, it is found that the stark effect could increases the polarization degree of a high pyramid dot by 5% by applying an electric field up to 200 KeV/cm.

碩士
國立臺灣大學
應用力學研究所
104
We studied the N-H...O=C and O-H...O=C type hydrogen bonds by substituting alkyl groups on amide and acid molecules. All the quantum chemistry calculations were performed at Gaussian 09 software to optimize individual keto or enol structures and search the transition state of proton transfer reaction. Meanwhile,we use the IRC(Intrinsic reaction coordinate) method to plot the reaction path in order to obtain the energy barrier. In addition, the PSI4 software was utilized through the SAPT method to decompose the intermolecular interaction into several physically meaningfull terms, to discuss the effect of alkyl groups on the proton transfer reaction. For the stack effect, we use amide and acid molecules in planar structures and use several vertically stacked layers to observe the effect of stacking on proton transfer reaction. Six-carbon ring on the outside is used to bond each layers, similar to the peripheral backbone in DNA double helix. The energy barrier of proton transfer under different stacking structures was also discussed. We also consider the hydration effect on amide and acid of proton transfer reaction. Recent studies have shown that water molecules could hamper direct proton transfer between nitrogenous bases, but it plays the role of proton donor and acceptor during the reaction. Therefore, water molecules can form hydrogen bonding network to be involved in the proton transfer process. In such cases we use amide and acid molecule as a simplified model for analysis. At the same time, the configuration of waters surrounding the dimer or clamping in the hydrogen bonds of the dimer has been discussed.

碩士
國立中山大學
物理學系研究所
103
Since the single layer graphene are observed by Andre Geim and Konstantin Novoselov, the quantum phenomena emerging from graphene as attracted many physicists’s attentions in the two dimensional lattice structure. One of the important quantum phenomena is the unconventional quantum Hall effect which the Hall plateau (Chern number pattern) does not show successive integers but only odd integers. However, there are some other problems to calculate the quantum Hall conductivity, such as the determination of the Chern number pattern from a specific lattice structure and the reduction of the computational time. Motivated by these issues, I use Yasuhiro Hatsugai’s topological approaches to investigate the quantum Hall effect of other lattices. I use Hatsugai’s method to calculate the quantum Hall conductivity in two different lattices: Kagomé and star lattices. I find that the Dirac-like regions of quantum Hall conductivity also exists in both Kagomé and star lattices, which is similar to graphene. Unlike the graphene, the star lattice shows complicated Chern number structure in the electron-hole like regions. Hopefully, the Chern number pattern of the star lattice predicted by us can be determined by experiments in the near future.

碩士
國立清華大學
物理學系
105
Ⅲ-nitride semiconductor heterostructures have been widely applied for blue and white light LEDs. However, the internal piezoelectric field can produce large quantum confined stark effects (QCSE), and reduce the light emission quantum efficiency. Here, we use InxGa1-xN (InGaN) nanorod heterostructures grown by plasma-assisted molecular-beam epitaxy (PA-MBE) for experimental investigation of QCSE. We have measured the micro photoluminescence (PL) spectra for the shift of PL peak energy versus optical pumping power intensity and time-resolved PL spectra for exciton measurements using InGaN nanodisk samples with different nanodisk thicknesses. We found that the thickness of InGaN nanodisk plays a significant role in the observation of QCSE.

Low-dimensional systems are an exciting platform for exploring new physics and realizing novel devices. The intriguing features, such as the existence of strongly bound multiparticle complexes and thickness-dependent band structures, enable us to utilize them to overcome many challenges faced by bulk materials and conceive new technologies. Since the isolation of graphene, the class of two-dimensional materials has grown tremendously. The array of materials one can choose from for implementing an idea is vast. Nevertheless, understanding the underlying physics is essential for utilizing these properties for real-life applications. Here, we explore the optical, electrical, and optoelectrical characteristics of heterostructures based on 2D layered systems. The strongly bound excitonic complexes hosted by monolayer transition metal dichalcogenide semiconductors (TMDC) are an excellent platform for probing many-body physics. The strong luminescence and a plethora of exciting properties make them a good candidate for applications such as single photon emitters and light-emitting diodes. In the first work, we explore new ways to tune the emission from these particles without compromising their luminescence. Using a high-quality graphene/hBN/WS2/hBN/Au vertical heterojunction, we demonstrate for the first time an out-of-plane electric field-driven change in the sign of the Stark shift from blue to red for four different excitonic species, namely, the neutral exciton, the charged exciton (trion), the charged biexciton, and the defect-bound exciton. We also find that the encapsulating environment of the monolayer TMDC plays a vital role in wave function spreading and hence in determining the magnitude of the blue Stark shift. We also provide a theoretical framework to understand the underlying physics better. The findings have important implications in probing many-body interaction in the two dimensions and developing layered semiconductor-based tunable optoelectronic devices. A significant advantage of the 2D material system is its robustness against lattice mismatch between the successive layers and the ability to extract exciting characteristics from the resultant system. The final system's behavior greatly depends on how the energy bands of the individual materials line up and can result in drastically different properties. In the second work, we demonstrate how an additional ultra-thin barrier layer modifies the properties of a black phosphorus (BP)/SnSe2 tunnel diode. While the system without the barrier layer showed a linear relationship between current and voltage, the additional barrier layer modified it to a highly nonlinear relation and exhibited negative differential resistance (NDR). Moreover, the tunnel diodes exhibited highly repeatable, ultra-clean, and gate tunable NDR characteristics with a signature of intrinsic oscillation and a large peak-to-valley current ratio (PVCR) of 3.6 at 300 K (4.6 at 7 K), making them suitable for practical applications. We then show that the thermodynamic stability of the van der Waals (vdW) tunnel diode circuit can be tuned from astability to bistability by altering the constraint by choosing a voltage or a current bias, respectively. After exploring the dynamics of the device, we assess its viability for designing systems with real-life applications. In the astable mode under voltage bias, we demonstrate a compact, voltage-controlled oscillator without needing an external tank circuit. In the bistable mode under current bias, we demonstrate a highly scalable, single element, a one-bit memory cell promising for dense random access memory applications in memory-intensive computation architectures. In the third work, we explore the usage of vdW materials for generating a cryptographically secure true random number generator. Such generators rely on external entropy sources for their indeterminism. Physical processes governed by the laws of quantum mechanics are excellent sources of entropy available in nature. However, extracting enough entropy from such systems for generating truly random sequences is challenging while maintaining the feasibility of the extraction procedure for real-world applications. Here, we design a compact and an all-electronic vdW heterostructure-based device capable of detecting discrete charge fluctuations for extracting entropy from physical processes and use it for the generation of independent and identically distributed (IID) true random sequences. Using the proposed scheme, we extract a record high value (> 0.98 bits/bit) of min-entropy. We demonstrate an entropy generation rate tunable over multiple orders of magnitude and show the persistence of the underlying physical process for temperatures ranging from cryogenic to ambient conditions. We verify the random nature of the generated sequences using tests such as the NIST SP 800-90B standard and other statistical measures and verify the suitability of our random sequence for cryptographic applications using the NIST SP 800-22 standard. The generated random sequences are then used to implement various randomized algorithms in real life without preconditioning steps. We then investigate how knowledge of the dynamics of optically generated carriers, ability to sense discrete charge fluctuation, and transport of carriers across vdW heterostructure can be combined to design a comprehensive system to detect single photons. Single-photon detectors (SPDs) are crucial in applications ranging from space and biological imaging to quantum communication and information processing. The SPDs operating at room temperature are particularly interesting to broader application spaces as the energy overhead introduced by cryogenic cooling can be avoided. Although silicon-based single photon avalanche diodes (SPADs) are well matured and operate at room temperature, the bandgap limitation restricts their operation at telecommunication wavelength (1550 nm) and beyond. On the other hand, InGaAs-based SPADs are sensitive to 1550 nm photons but suffer from relatively lower efficiency, high dark count rate, afterpulsing probability, and pose hazards to the environment from the fabrication process. By coupling a low bandgap (~350 meV) absorber (black phosphorus) to a sensitive van der Waals probe capable of detecting discrete electron fluctuation, we demonstrate a room-temperature single-photon detector. While the device is capable of covering up to a wavelength of ~3.5 um, we optimize the device for operation at 1550 nm and demonstrate an overall quantum efficiency of 21.4% (estimated as 42.8% for polarized light) and a minimum dark count of ~720 Hz at room temperature.